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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2019

Reverse Monte Carlo modeling for low-dimensional systems

Reverse Monte Carlo (RMC) is one of the commonly used approaches for modeling total scattering data. However, to extend the capability of the RMC method for refining the structure of nanomaterials, the dimensionality and finite size need to be considered when calculating the pair distribution function (PDF). To achieve this, the simulation box must be set up to remove the periodic boundary condition in one, two or three of the dimensions. This then requires a correction to be applied for the difference in number density between the real system and the simulation box. In certain circumstances an analytical correction for the uncorrelated pairings of atoms is also applied. The validity and applicability of our methodology is demonstrated by applying the algorithms to simulate the PDF patterns of carbon systems with various dimensions, and also by using them to fit experimental data of CuO nanoparticles. This alternative approach for characterizing the local structure of nano-systems with the total scattering technique will be made available via the RMCProfile package. The theoretical formulation and detailed explanation of the analytical corrections for low-dimensional systems – 2D nanosheets, 1D nanowires and 0D nanoparticles – is also given.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Integrating machine learning interatomic potentials with hybrid reverse Monte Carlo structure refinements in RMCProfile

Structure refinement with reverse Monte Carlo (RMC) is a powerful tool for interpreting experimental diffraction data. To ensure that the under-constrained RMC algorithm yields reasonable results, the hybrid RMC approach applies interatomic potentials to obtain solutions that are both physically sensible and in agreement with experiment. To expand the range of materials that can be studied with hybrid RMC, we have implemented a new interatomic potential constraint in RMCProfile that grants flexibility to apply potentials supported by the Large-scale Atomic/Molecular Massively Parallel Simulator ( LAMMPS ) molecular dynamics code. This includes machine learning interatomic potentials, which provide a pathway to applying hybrid RMC to materials without currently available interatomic potentials. To this end, we present a methodology to use RMC to train machine learning interatomic potentials for hybrid RMC applications.

Cuillier, Paul↗
DOE OSTI2016

Fullrmc, a rigid body reverse monte carlo modeling package enabled with machine learning and artificial intelligence

Here, a new Reverse Monte Carlo (RMC) package ‘fullrmc’ for atomic or rigid body and molecular, amorphous or crystalline materials is presented. fullrmc main purpose is to provide a fully modular, fast and flexible software, thoroughly documented, complex molecules enabled, written in a modern programming language (python, cython ,C and C++ when performance is needed) and complying to modern programming practices. fullrmc approach in solving an atomic or molecular structure is different from existing RMC algorithms and software. In a nutshell, traditional RMC methods and software randomly adjust atom positions until the whole system has the greatest consistency with a set of experimental data. In contrast, fullrmc applies smart moves endorsed with reinforcement machine learning to groups of atoms. While fullrmc allows running traditional RMC modelling, the uniqueness of this approach resides in its ability to customize grouping atoms in any convenient way with no additional programming efforts and to apply smart and more physically meaningful moves to the defined groups of atoms. Also fullrmc provides a unique way with almost no additional computational cost to recur a group’s selection, allowing the system to go out of local minimas by refining a group’s position or exploring through and beyond not allowed positions and energy barriers the unrestricted three dimensional space around a group.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2016

The structure of molten CuCl: Reverse Monte Carlo modeling with high-energy X-ray diffraction data and molecular dynamics of a polarizable ion model

The results of the structural properties of molten copper chloride are reported from high-energy X-ray diffraction measurements, reverse Monte Carlo modeling method, and molecular dynamics simulations using a polarizable ion model. The simulated X-ray structure factor reproduces all trends observed experimentally, in particular the shoulder at around 1 Å{sup −1} related to intermediate range ordering, as well as the partial copper-copper correlations from the reverse Monte Carlo modeling, which cannot be reproduced by using a simple rigid ion model. It is shown that the shoulder comes from intermediate range copper-copper correlations caused by the polarized chlorides.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

RMCProfile7 : reverse Monte Carlo for multiphase systems

This work introduces a completely rewritten version of the programRMCProfile(version 7), big-box, reverse Monte Carlo modelling software for analysis of total scattering data. The major new feature ofRMCProfile7is the ability to refine multiple phases simultaneously, which is relevant for many current research areas such as energy materials, catalysis and engineering. Other new features include improved support for molecular potentials and rigid-body refinements, as well as multiple different data sets. An empirical resolution correction and calculation of the pair distribution function as a back-Fourier transform are now also available.RMCProfile7is freely available for download at https://rmcprofile.ornl.gov/.

Chemistry↗
DOE OSTI2023

Study of beyond nearest-neighbor environment and intermediate-range order in a sodium aluminosilicate geopolymer using Reverse Monte Carlo modeling

A large scale three-dimensional structural model of a geopolymer with an approximate composition of NaAlSi 2 O 6 .5.5H 2 O obtained by Reverse Monte Carlo (RMC) modeling based on experimental high-energy x-ray diffraction is presented for the first time in order to obtain information regarding beyond nearest-neighbor environment and intermediate-range order (IRO). RMC model exhibits a three-dimensional network consisting of randomly cross-linked AlO 4 and SiO 4 tetrahedral units with uniformly distributed Na atoms and H 2 O molecules. The bond angle distributions, i.e. T-O-T, O-T-O and Na-O-Na angles, are somewhat distorted with lower values compared to analogous crystal systems. The origin of the first peak in the structure factor indicating IRO is investigated using the partial structure factors; Na-Na, Si-Na, Al-Si, O-H, and H-H atom pairs are found to be the main contributors. Ring size distribution analysis demonstrates that the structure mainly involves 6-, 7- and 8-membered rings. Finally, the coherence length of these IRO characteristics is ~10.3 Å.

36 MATERIALS SCIENCE↗
DOE OSTI2021

rmc-discord : reverse Monte Carlo refinement of diffuse scattering and correlated disorder from single crystals

A user-friendly program has been developed to analyze diffuse scattering from single crystals with the reverse Monte Carlo method. The approach allows for refinement of correlated disorder from atomistic supercells with magnetic or structural (occupational and/or displacive) disorder. The program is written in Python and optimized for performance and efficiency. Refinements of two user cases obtained with legacy neutron-scattering data demonstrate the effectiveness of the approach and the developed program. It is shown with bixbyite, a naturally occurring magnetic mineral, that the calculated three-dimensional spin-pair correlations are resolved with finer real-space resolution compared with the pair distribution function calculated directly from the reciprocal-space pattern. With the triangular lattice Ba 3 Co 2 O 6 (CO 3 ) 0.7 , refinements of occupational and displacive disorder are combined to extract the one-dimensional intra-chain correlations of carbonate molecules that move toward neighboring vacant sites to accommodate strain induced by electrostatic interactions. The program is packaged with a graphical user interface and extensible to serve the needs of single-crystal diffractometer instruments that collect diffuse-scattering data.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2017

Structure of Se-Te glasses studied using neutron, X-ray diffraction and reverse Monte Carlo modelling

Pulsed neutron diffraction and synchrotron X-ray diffraction measurements were performed on Se{sub 100-x}Te{sub x} bulk glasses with x=10, 20, 30 and 40. The coordination numbers obtained from the diffraction results demonstrate that Se and Te atoms are twofold coordinated and the glass structure is formed by the chain network. The three-dimensional structure model for Se{sub 60}Te{sub 40} glass obtained by using reverse Monte Carlo modelling shows that the alternating arrangements of Se and Te atoms compose the major part of the chain clusters but several other fragments such as Se{sub n} chains and Te-Te dimers are also present in large numbers. The chain clusters have geometrically disordered forms and the interchain atomic order is different from those in the crystal structures of trigonal Se and trigonal Te. - Graphical abstract: Coordination environment in Se{sub 60}Te{sub 40} glass.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Structural analysis of WO 3 -TeO 2 glasses by neutron, high energy X-ray diffraction, reverse Monte Carlo simulations and XANES

The structure of WO 3 -TeO 2 glasses containing 15, 20 and 25 mol% WO 3 are studied by neutron diffraction (ND), high energy X-ray diffraction (XRD) and X-ray Absorption Near Edge spectroscopy (XANES). The short-range structural properties of glasses i.e. Te-O and W-O speciation, coordination number distributions, bond-lengths, and the O-Te-O, O-W-O and O-O-O bond angle distributions in the glass network are determined by the Reverse Monte Carlo (RMC) simulations of the ND and XRD data. RMC technique successfully determined all partial pair correlation functions and the coordination number distributions revealed that glass network consists predominantly of TeO 4 and WO 4 units with small amounts of triangular, penta and hexa co-ordinated units. The average W-O and Te-O bond lengths are in the ranges: 1.69-1.75 +/- 0.01 angstrom and 1.99-2.00 +/- 0.01 angstrom respectively. Both W-O and Te-O correlation peaks are asymmetrical, that indicate a distribution of their bond lengths in the respective structural units. The O-Te-O bond angle distribution has a peak at 107 +/- 2 degrees. Similarly the O-W-O bond angle distribution has a peak at 108 +/- 5 degrees. On increasing the WO3 concentration from 15 to 25 mol%, the average Te-O coordination number decreases from 3.80 to 3.61 +/- 0.02 due to the structural transformation: TeO 4 → TeO 3 , similarly the W-O coordination also decreases and is in the range: 3.79-3.67 +/- 0.02. XANES studies found that the oxidation state of Te and W ions in the glasses are 4 + and 6 + respectively.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Radiative Heat Transfer Calculation on 16384 GPUs Using a Reverse Monte Carlo Ray Tracing Approach with Adaptive Mesh Refinement

Modeling thermal radiation is computationally challenging in parallel due to its all-to-all physical and resulting computational connectivity, and is also the dominant mode of heat transfer in practical applications such as next-generation clean coal boilers, being modeled by the Uintah framework. However, a direct all-to-all treatment of radiation is prohibitively expensive on large computers systems whether homogeneous or heterogeneous. DOE Titan and the planned DOE Summit and Sierra machines are examples of current and emerging GPU-based heterogeneous systems where the increased processing capability of GPUs over CPUs exacerbates this problem. These systems require that computational frameworks like Uintah leverage an arbitrary number of on-node GPUs, while simultaneously utilizing thousands of GPUs within a single simulation. We show that radiative heat transfer problems can be made to scale within Uintah on heterogeneous systems through a combination of reverse Monte Carlo ray tracing (RMCRT) techniques combined with AMR, to reduce the amount of global communication. In particular, significant Uintah infrastructure changes, including a novel lock and contention-free, thread-scalable data structure for managing MPI communication requests and improved memory allocation strategies were necessary to achieve excellent strong scaling results to 16384 GPUs on Titan.

Computer Science↗
DOE OSTI2017

Oxygen-storage behavior and local structure in Ti-substituted YMnO{sub 3}

Hexagonal manganates RMnO{sub 3} (R=Y, Ho, Dy) have been recently shown to exhibit oxygen-storage capacities promising for three-way catalysts, air-separation, and related technologies. Here, we demonstrate that Ti substitution for Mn can be used to chemically tune the oxygen-breathing properties of these materials towards practical applications. Specifically, Y(Mn{sub 1−x}Ti{sub x})O{sub 3} solid solutions exhibit facile oxygen absorption/desorption via reversible Ti{sup 3+}↔Ti{sup 4+} and Mn{sup 3+}↔Mn{sup 4+} reactions already in ambient air at ≈400 °C and ≈250 °C, respectively. On cooling, the oxidation of both cations is accompanied by oxygen uptake yielding a formula YMn{sup 3+}{sub 1−x-y}Mn{sup 4+}{sub y}Ti{sup 4+}{sub x}O{sub 3+δ}. The presence of Ti promotes the oxidation of Mn{sup 3+} to Mn{sup 4+}, which is almost negligible for YMnO{sub 3} in air, thereby increasing the uptake of oxygen beyond that required for a given Ti{sup 4+} concentration. The reversibility of the redox reactions is limited by sluggish kinetics; however, the oxidation process continues, if slowly, even at room temperature. The extra oxygen atoms are accommodated by the large interstices within a triangular lattice formed by the [MnO{sub 5}] trigonal bipyramids. According to bond distances from Rietveld refinements using the neutron diffraction data, the YMnO{sub 3} structure features under-bonded Mn and even more severely under-bonded oxygen atoms that form the trigonal bases of the [MnO{sub 5}] bipyramids. The tensile bond strain around the 5-fold coordinated Mn site and the strong preference of Ti{sup 4+}(and Mn{sup 4+}) for higher coordination numbers likely provide driving forces for the oxidation reaction. Reverse Monte Carlo refinements of the local atomic displacements using neutron total scattering revealed how the excess oxygen atoms are accommodated in the structure by correlated local displacements of the host atoms. Large displacements of the under-bonded host oxygen atoms play a key part in this lattice-relaxation process, facilitating reversible exchange of significant amounts of oxygen with atmosphere. - Graphical abstract: Concurrent redox reactions involving Ti and Mn yield facile absorption/desorption of excess oxygen. - Highlights: • Concurrent redox reactions involving Ti and Mn yield oxygen absorption/desorption. • Excess oxygen is accommodated as interstitials via correlated atomic shifts. • Oxygen breathing is facilitated by the under-bonding of host Mn and O atoms.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Role of Short-Range Chemical Ordering in (GaN) 1– x (ZnO) x for Photodriven Oxygen Evolution

(GaN) 1–x (ZnO) x (GZNO) is capable of visible-light driven water splitting, but its bandgap at x ≤ 0.15 (>2.7 eV) results in poor visible-light absorption. Unfortunately, methods to narrow its bandgap by incorporating higher ZnO concentrations are accompanied by extensive Urbach tailing near the absorption-edge, which is indicative of structural disorder or chemical inhomogeneities. We evaluated whether this disorder is intrinsic to the bond-length distribution in GZNO or is a result of defects introduced from the loss of Zn during nitridation. Here, the synthesis of GZNO derived from layered double hydroxide (LDH) precursors is described which minimizes Zn loss and chemical inhomogeneities and enhances visible-light absorption. The average and local atomic structures of LDH-derived GZNO were investigated using X-ray and neutron scattering and are correlated with their oxygen evolution rates. An isotope-contrasted neutron-scattering experiment was conducted in conjunction with reverse Monte Carlo (RMC) simulations. We showed that a bond-valence bias in the RMC refinements reproduces the short-range ordering (SRO) observed in structure refinements using isotope-contrasted neutron data. The findings suggest that positional disorder of cation–anion pairs in GZNO partially arises from SRO and influences local bond relaxations. Furthermore, particle-based oxygen evolution reactions (OERs) in AgNO 3 solution reveal that the crystallite size of GZNO correlates more than positional disorder with oxygen evolution rate. In conclusion, these findings illustrate the importance of examining the local structure of multinary photocatalysts to identify dominant factors in particulate-based photodriven oxygen evolution.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Metal–Carbodithioate-Based 3D Semiconducting Metal–Organic Framework: Porous Optoelectronic Material for Energy Conversion

Solar energy conversion requires the working compositions to generate photoinduced charges with high potential and the ability to deliver charges to the catalytic sites and/or external electrode. These two properties are typically at odds with each other and call for new molecular materials with sufficient conjugation to improve charge conductivity but not as much conjugation as to overly compromise the optical band gap. In this work, we developed a semiconducting metal-organic framework (MOF) prepared explicitly through metal-carbodithioate"(-CS 2 ) n M" linkage chemistry, entailing augmented metal-linker electronic communication. The stronger ligand field and higher covalent character of metal-carbodithioate linkages-when combined with spirofluorene-derived organic struts and nickel-(II) ion-based nodes-provided a stable, semiconducting 3D-porous MOF, Spiro-CS 2 Ni. This MOF lacks long-range ordering and is defined by a flexible structure with non-aggregated building units, as suggested by reverse Monte Carlo simulations of the pair distribution function obtained from total scattering experiments. The solvent-removed "closed pore"material recorded a Brunauer-Emmett-Teller area of similar to 400m 2 /g, where the "open pore" form possesses90 wt % solvent-accessible porosity. Electrochemical measurements suggest that Spiro-CS 2 Ni possesses a band gap of 1.57 eV(sigma = 10 -7 S/cm at -1.3 V bias potential),which can be further improved by manipulating the d-electron configuration through an axial coordination (ligand/substrate), the latter of which indicates usefulness as an electrocatalyst and/or a photoelectrocatalyst(upon substrate binding). Transient-absorption spectroscopy reveals a long-lived photo-generated charge-transfer state (τ CR = 6.5 mu s) capable of chemical transformation under a biased voltage. Spiro-CS 2 Ni can endure a compelling range of pH(1-12 for weeks) and hours of electrochemical and photoelectrochemical conditions in the presence of water and organic acids. We believe this work provides crucial design principles for low-density, porous,light-energy-conversion materials.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Pressure cells for in situ neutron total scattering: time and real-space resolution during deuterium absorption

In situ gas-loading sample holders for two-dimensionally arranged detectors in time-of-flight neutron total scattering experiments have been developed to investigate atomic arrangements during deuterium absorption using time and real-space resolution. A single-crystal sapphire container was developed that allows conditions of 473 K and 10 MPa hydrogen gas pressure. High-resolution transient measurements detected deuterium absorption by palladium that proceeded within a few seconds. A double-layered container with thick- and thin-walled vanadium allowed conditions of 423 K and 10 MPa hydrogen gas pressure. The deuterium occupation sites of a lanthanum–nickel–aluminium alloy are discussed in detail on the basis of real-space high-resolution data obtained from in situ neutron scattering measurements and reverse Monte Carlo structural modeling.

08 HYDROGEN↗
DOE OSTI2022

Describing the Influence of Ball-milling on the Amorphization of Flubendazole Using the PDF and RMC Methods with X-ray Powder Diffraction Data

Flubendazole (FBZ) is a poorly water-soluble drug, and different methodologies have been proposed to improve its oral bioavailability. Obtaining the amorphous drug phase is an alternative to improve its water solubility. Several techniques for drug amorphization, such as spray drying, lyophilization, melt quenching, solvent-evaporation, and ball milling, can yield various types of structural disorder and possibly render variations in physicochemical properties. Herein, we focus on evaluating the influence of the ball-milling process on the amorphization of FBZ. The characterization of the average global and local structures before, during, and after the milling process is described by sequential Rietveld refinements, pair distribution function analysis, and the Reverse Monte Carlo method. In conclusion, we show that preserving the local structure (nearest molecules) can be responsible for avoiding the fast structure recrystallization commonly observed when using the solvent-evaporation process for the studied drug.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2022

Ferroelectric Ordering in Nanosized PbTiO 3

The insight into the three-dimensional configuration of ferroelectric ordering in ferroelectric nanomaterials is motivated by the application of the development of functional nanodevices and the structural designing. However, the atomic deciphering of the spatial distribution of ordered structure remains challenging for the limitation of dimension and probing techniques. Here, in this paper, a neutron pair distribution function (nPDF) was utilized to analyze the spontaneous polarization distribution of zero-dimensional PbTiO 3 nanoparticles in three dimensions, via the application of reverse Monte Carlo (RMC) modeling. The comprehensive identification with transmission electron microscopy verified the linear characteristics of polarization along the c-axis in the main body, while electric polarization distribution on the surface was enhanced abnormally. In addition, the correlation of dipole vectors extending to three unit cells below the surface is retained. This work shows an application of the micro/macroscale information to effectively decode the polarization structure of nanoferroelectrics, providing new views of designing nanoferroelectric devices.

36 MATERIALS SCIENCE↗